• •
陈贵梅1,2(), 谢雨芸1,2, 杨有威1,2, 高艳1,2, 王春英1,2(
)
收稿日期:
2024-04-03
修回日期:
2024-07-17
出版日期:
2024-07-23
通讯作者:
王春英
作者简介:
陈贵梅(2001-),女,硕士研究生,2380164332@qq.com
基金资助:
Guimei CHEN1,2(), Yuyun XIE1,2, Youwei YANG1,2, Yan GAO1,2, Chunying WANG1,2(
)
Received:
2024-04-03
Revised:
2024-07-17
Online:
2024-07-23
Contact:
Chunying WANG
摘要:
采用铜铁类普鲁士蓝衍生物(CunFe1-PBAs)活化过一硫酸盐(PMS)降解罗丹明B(RhB),考察铁铜摩尔比、催化剂投加量、PMS与RhB的摩尔比、起始pH和水中常见离子对RhB降解的影响。结果表明:Cu2Fe1-PBAs可以有效活化PMS降解RhB。在RhB浓度为20 mg/L,Cu2Fe1-PBAs用量为0.6 g/L,PMS浓度为0.513 g/L,碱性条件时最有利于RhB降解。NO3-、HCO3-、Cl- 促进RhB的降解,SO42-抑制RhB的降解。硫酸根自由基(SO4-·)、羟基自由基(·OH)、单线态氧(¹O₂)和超氧自由基(·O2-)均参与Cu2Fe1-PBAs活化PMS降解RhB反应过程中。
中图分类号:
陈贵梅, 谢雨芸, 杨有威, 高艳, 王春英. 类普鲁士蓝衍生物活化过一硫酸盐降解罗丹明B研究[J]. 化工学报, DOI: 10.11949/0438-1157.20240371.
Guimei CHEN, Yuyun XIE, Youwei YANG, Yan GAO, Chunying WANG. Degradation of Rhodamine B by Peroxymonosulfate activated by Prussian blue analogue derivatives[J]. CIESC Journal, DOI: 10.11949/0438-1157.20240371.
图1 铁铜摩尔比例对RhB降解效果的影响注:实验条件:[Cu2Fe1-PBAs]0=400 mg/L; [PMS]0=500 mg/L; pH0=5.16; [RhB]0=20 mg/L; 反应温度为25±2 ◦C
Fig.1 Effect of molar ratio of iron to copper on degradation of RhBReaction conditions: [Cu2Fe1-PBAs]0=400 mg/L; [PMS]0=500 mg/L; pH0=5.16; [RhB]0=20 mg/L; Temperature 25±2 ◦C
催化方式 | 催化剂浓度(mg/L) | 初始浓度(mg/L) | PMS(mg/L) | pH | 反应时间(min) | 去除率(%) | 文献来源 | |
---|---|---|---|---|---|---|---|---|
Cu2Fe1-PBAs | 600 | 20.0 | 513 | 5.16 | 30 | 92.72 | 本文 | |
磁性茶渣炭 | 213 | 40.0 | 302 | 5 | 80 | 98 | [ | |
紫外光下施氏矿物 | 500 | 4.79 | 307 | —— | 45 | 93.7 | [ | |
黄铁矿 | 1000 | 20 | 307 | 5 | 180 | 99 | [ | |
铁酸铜 | 100 | 2.39 | 61 | —— | 30 | 88.87 | [ | |
氧化铜纳米颗粒 | 500 | 50 | 614 | 7.5 | 60 | 93.38 | [ | |
兔粪生物炭 | 600 | 25 | 400 | —— | 40 | 98 | [ |
表1 其他可活化过一硫酸盐降解RhB的实验对比
Table 1 Comparison of other experiments for the degradation of RhB by activated peroxymonosulfate
催化方式 | 催化剂浓度(mg/L) | 初始浓度(mg/L) | PMS(mg/L) | pH | 反应时间(min) | 去除率(%) | 文献来源 | |
---|---|---|---|---|---|---|---|---|
Cu2Fe1-PBAs | 600 | 20.0 | 513 | 5.16 | 30 | 92.72 | 本文 | |
磁性茶渣炭 | 213 | 40.0 | 302 | 5 | 80 | 98 | [ | |
紫外光下施氏矿物 | 500 | 4.79 | 307 | —— | 45 | 93.7 | [ | |
黄铁矿 | 1000 | 20 | 307 | 5 | 180 | 99 | [ | |
铁酸铜 | 100 | 2.39 | 61 | —— | 30 | 88.87 | [ | |
氧化铜纳米颗粒 | 500 | 50 | 614 | 7.5 | 60 | 93.38 | [ | |
兔粪生物炭 | 600 | 25 | 400 | —— | 40 | 98 | [ |
图2 Cu2Fe1-PBAs投加量对RhB降解的影响(a)和一级动力学模拟(b)注:Reaction conditions: [Cu2Fe1-PBAs]0=200-600 mg/L; [PMS]0=513 mg/L; pH0=5.16; [RhB]0=20 mg/L; Temperature 25±2 ◦C实验条件:[Cu2Fe1-PBAs]0=200-800 mg/L; [PMS]0=500 mg/L; pH0=5.16; [RhB]0=20 mg/L; 反应温度为25±2 ◦C
Fig.2 Effect of Cu2Fe1-PBAs dosage on RhB degradation (a) and the corresponding curves of pseudo-first order reaction kinetics (b)
图3 PMS投加量对RhB降解的影响(a)和一级动力学模拟(b)注:Reaction conditions: [Cu2Fe1-PBAs]0=600 mg/L; [PMS]0=128-1026 mg/L; pH0=5.16; [RhB]0=20 mg/L; Temperature 25±2 ◦C实验条件:[Cu2Fe1-PBAs]0=600 mg/L; [PMS]0=128-1026 mg/L; pH0=5.16; [RhB]0=20 mg/L; 反应温度为25±2 ◦C
Fig.3 Effect of PMS Dosage on RhB degradation (a) and the corresponding curves of pseudo-first order reaction kinetics (b)
图4 PMS的反应剩余注:实验条件:[Cu2Fe1-PBAs]0=600 mg/L; [PMS]0=128-1026 mg/L; pH0=5.16; [RhB]0=20 mg/L; 反应温度为25±2 ◦C
Fig.4 Residual degradation of PMSReaction conditions: [Cu2Fe1-PBAs]0=600 mg/L; [PMS]0=128-1026 mg/L; pH0=5.16; [RhB]0=20 mg/L; Temperature 25±2 ◦C
图5 催化剂四次循环催化效果注:实验条件:[Cu2Fe1-PBAs]0=600 mg/L; [PMS]0=513 mg/L; pH0=5.16; [RhB]0=20 mg/L; 反应温度为25±2 ◦C
Fig.5 Catalytic effect of four cycles of catalystReaction conditions: [Cu2Fe1-PBAs]0=600 mg/L; [PMS]0=513 mg/L; pH0= 5.16; [RhB]0=20 mg/L; Temperature 25±2 ◦C
图6 起始pH对RhB降解的影响注:实验条件:[Cu2Fe1-PBAs]0=600 mg/L; [PMS]0=513 mg/L; pH0=3-11; [RhB]0=20 mg/L; 反应温度为25±2 ◦C
Fig.6 Effect of initial pH on RhB degradationReaction conditions: [Cu2Fe1-PBAs]0=600 mg/L; [PMS]0=513 mg/L; pH0= 3-11; [RhB]0=20 mg/L; Temperature 25±2 ◦C
图7 紫外可见光光谱(a)不同初始pH反应30min后溶液的谱图; (b) 初始pH=11在不同反应时间下的谱图(实验条件:[Cu2Fe1-PBAs]0=600 mg/L; [PMS]0=513 mg/L; pH0=3-11; [RhB]0=20 mg/L; 反应温度为25±2 ◦C)
Fig.7 Ultraviolet-visible spectrum of catalytic degradation of RhB system at each pH after 30 min (a) and pH=11 with different reaction time (Reaction conditions: [Cu2Fe1-PBAs]0=600 mg/L; [PMS]0=513 mg/L; pH0= 3-11; [RhB]0=20 mg/L; Temperature 25±2 ◦C)
图8 共存阴离子对RhB降解的影响注:实验条件:共存阴离子浓度为5 mM; [Cu2Fe1-PBAs]0=600 mg/L; [PMS]0=513 mg/L; pH0=5.16; [RhB]0=20 mg/L; 反应温度为25±2 ◦C
Fig.8 Effect of co-existing anions on RhB degradationReaction conditions: coexisting anion 5 mM;[Cu2Fe1-PBAs]0=600 mg/L; [PMS]0=513 mg/L; pH0= 5.16; [RhB]0=20 mg/L; Temperature 25±2 ◦C
图9 (a)不同活性组分猝灭剂对RhB降解的影响(实验条件:猝灭剂浓度为50-1000 mM; [Cu2Fe1-PBAs]0= 600 mg/L; [PMS]0=513 mg/L; pH0=5.16; [RhB]0=20 mg/L; 反应温度为25±2 ◦C);(b)TEMP的电子顺磁共振谱和(c,d) DMPO的电子顺磁共振谱
Fig.9 (a)Effects of different radical scavengers on RhB degradation (Reaction conditions: radical scavengers 50-1000 mM;[Cu2Fe1-PBAs]0=600 mg/L; [PMS]0=513 mg/L; pH0=5.16; [RhB]0=20 mg/L; Temperature 25±2 ◦C); EPR spectrums of (b)TEMP and (c,d)DMPO
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